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Indirect Z-scheme heterojunction of NH2-MIL-125(Ti) MOF/g-C3N4 nanocomposite with RGO solid electron mediator for efficient photocatalytic CO2 reduction to CO and CH4
Journal of Environmental Chemical Engineering ( IF 7.4 ) Pub Date : 2021-05-01 , DOI: 10.1016/j.jece.2021.105600
Riyadh Ramadhan Ikreedeegh , Muhammad Tahir

Well-designed Z-scheme photocatalyst of NH2-MIL-125(Ti) MOF coupled g-C3N4 with RGO mediator synthesized with a facile hydrothermal method has been investigated for stimulating photocatalytic CO2 reduction under visible light. The amino-functionalized Ti-based MOF boosted the photocatalytic efficiency due to its high surface area and porous structure. Moreover, the NH2-MIL-125(Ti) MOF has a great ability for CO2 gas adsorption. The novel RGO-linked g-C3N4/NH2-MIL-125(Ti) nanocomposite exhibited efficient photocatalytic CO2 conversion to CH4 and CO. The experimental results showed that CO was the predominant reaction product with a production of 383.79 μmol g-1 achieved after 4 h irradiation which is 5 and 2.5 times higher compared to pure g-C3N4 and zero-MOF g-C3N4-RGO composite, respectively. However, the composite also exhibited a CH4 evolution of 13.8 μmol g-1. The amino functionality provided the MOF with antenna-like reaction sites with high affinity to CO2 molecules which improved the photocatalytic reduction of CO2 towards high CO production selectivity. An effective spatial separation and transfer of photogenerated charge carriers was also obtained as a result of RGO incorporation which constructed an effective Z-scheme bridge for the transfer of charges and limiting the high recombination rate of g-C3N4. The stability analysis of the newly developed composite revealed a continuous production of CO and CH4 in multiple cycles without any obvious deactivation under visible light. This work provides a new approach for the construction of Z-scheme heterojunction composites that would be beneficial for further investigations in selective CO2 conversion to solar fuels.



中文翻译:

NH 2 -MIL-125(Ti)MOF / gC 3 N 4纳米复合物与RGO固体电子介体的间接Z型异质结,可有效地将CO 2光催化还原为CO和CH 4

研究了精心设计的NH 2 -MIL-125(Ti)MOF的g-C 3 N 4偶联Z-光催化剂,并用简便的水热法合成了RGO介体,以促进可见光下的光催化CO 2还原。氨基官能化的Ti基MOF由于其高表面积和多孔结构而提高了光催化效率。此外,NH 2 -MIL-125(Ti)MOF具有很强的CO 2气体吸附能力。新型的RGO连接的gC 3 N 4 / NH 2 -MIL-125(Ti)纳米复合材料表现出有效的光催化CO 2转化为CH 4的能力实验结果表明,CO是主要的反应产物,辐照4 h后产生的产量为383.79μmolg -1 ,是纯gC 3 N 4和零-MOF gC 3 N 4的5和2.5倍-RGO复合材料。然而,该复合物还表现出13.8μmolg -1的CH 4析出。氨基官能团使MOF具有与CO 2分子高度亲合的天线状反应位点,从而改善了CO 2的光催化还原向高CO生产选择性的方向发展。通过掺入RGO,还获得了光生电荷载流子的有效空间分离和转移,该结构为电荷转移和限制gC 3 N 4的高重组率构建了有效的Z-方案桥。对新开发的复合材料的稳定性分析表明,在可见光下,在多个循环中连续生产CO和CH 4,而没有任何明显的失活。这项工作为Z型异质结复合材料的构造提供了一种新方法,这将有助于进一步研究选择性CO 2转化为太阳能的研究。

更新日期:2021-05-02
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